文献类型：期刊文献

英文题名：Operando and Kinetic Study of Low-Temperature, Lean-Burn Methane Combustion over a Pd/γ-Al₂O₃ Catalyst

作者：Xu, Jing[1];Ouyang, Like[1];Mao, Wei[1];Yang, Xue-Jing[1];Xu, Xin-Chao[1];Su, Jun-Jie[1];Zhuang, Ting-Zhou[1];Li, Hui[2];Han, Yi-Fan[1]

机构：[1]E China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[2]Shanghai Normal Univ, Dept Chem, Shanghai 200234, Peoples R China

年份：2012

卷号：2

期号：2

起止页码：261

外文期刊名：ACS CATALYSIS

收录：;WOS:【SCI-EXPANDED(收录号:WOS:000299967500008)】；

基金：The authors are grateful for support from the Chinese Education Ministry 111 project (1308021), the National Natural Science Foundation of China (21176071, 21106041, 20973113), the Shanghai PuJiang Talent Program (2010/10PJ1402500, 2011/11PJ1402400), the Innovation Program of the Shanghai Municipal Education Commission (11ZZ52, 11ZZ051), the Shanghai Natural Science Foundation (11ZR1408400), the Opening Project Program of the State Key Laboratory of Chemical Engineering (SKL-ChE-10C05), the program of the Science and Technology Commission of the Shanghai Municipality (11JC1402700), the Creative Team Development Project of the Ministry of Education (IRT0721), and the Fundamental Research Funds for the Central Universities.

语种：英文

外文关键词：kinetics; low-temperature methane combustion; operando spectroscopy; Raman; in situ DRIFTS; Pd/gamma-Al2O3; catalyst

摘要：Operando and kinetic studies of lean-burn methane combustion were preformed on a Pd(3.3 wt %)/gamma-Al2O3 catalyst in a low temperature range of 473-673 K. The reaction order with respect to oxygen decreased with temperature, and the order with respect to methane remained constant. The working catalyst is characterized using operando Raman spectroscopy and in situ diffuse reflectance infrared Fourier transform spectroscopy of CO adsorption (DRIFTS), and the Pd chemical states were measured with X-ray photoelectron spectroscopy (XPS). Partial oxidation of Pd atoms during reaction was identified by Raman and XPS spectroscopies. In particular, the DRIFT spectra revealed that similar to 45% of Pd atoms at the top layers were transferred into PdOx species above 523 K. The reaction was assumed to occur primarily on the metallic Pd sites below 673 K, proceeding through the Langmuir-Hinshelwood mechanism, and Pd oxide may affect the adsorption and activation of reactants.